Issue 34, 2021

Using nickel to fold discrete synthetic macromolecules into single-chain nanoparticles

Abstract

Macromolecules found in Nature display a precise control over the primary as well as higher ordered architectures. To mimic the folding found in Nature, we herein demonstrate the design and characterization of single-chain nanoparticles that are formed by the folding of sequence-defined macromolecules with metal ions. The study showcases the influence of the loop size of such precision macromolecules on their relative hydrodynamic radius. The sequence-defined structures are fabricated using thiolactone chemistry, where two picolyl moieties are installed forming a valuable ligand system for subsequent metal complexation. Next, metal ions such as Ni(II) and Cu(II) ions are introduced to fold the unimers into sequence-defined single-chain nanoparticles (SD-SCNPs). After proving the successful complexation using a trimer, a systematic study is conducted altering the distance between the respective ligands by incorporating variable numbers of non-functionalized spacer units. Finally, the loop size formation of the SD-SCNPs is evidenced by DOSY measurements. The result indicates that the positioning of the ligands plays a crucial role on the compaction process and, more specifically, on the final size of the SD-SCNP. In addition, molecular dynamics (MD) simulations show the effects of the sequence and Ni(II) complexation on the structure and compaction of the SD-SCNPs, and highlight the differences of the nanoparticles’ shape when varying the number of spacer units. Finally, the system is further expanded to a dodecamer and even a heptadecamer with drastically decreased hydrodynamic radii after compaction.

Graphical abstract: Using nickel to fold discrete synthetic macromolecules into single-chain nanoparticles

Supplementary files

Article information

Article type
Paper
Submitted
19 Feb 2021
Accepted
21 Jun 2021
First published
21 Jun 2021

Polym. Chem., 2021,12, 4924-4933

Using nickel to fold discrete synthetic macromolecules into single-chain nanoparticles

M. A. Reith, S. Kardas, C. Mertens, M. Fossépré, M. Surin, J. Steinkoenig and F. E. Du Prez, Polym. Chem., 2021, 12, 4924 DOI: 10.1039/D1PY00229E

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